Biomass burning influence on high-latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations
Biomass burning influence on high-latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations
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DOI：
10.5194/acp-15-6047-2015
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发表时间：
2014-09
影响因子：
6.3
通讯作者：
S. Arnold;L. Emmons;S. Monks;K. Law;D. Ridley;S. Turquety;S. Tilmes;Jennie L. Thomas;I. Bouarar;J. Flemming;V. Huijnen;J. Mao;B. Duncan;S. Steenrod;Y. Yoshida;J. Langner;Y. Long
中科院分区：
文献类型：
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作者：
S. Arnold;L. Emmons;S. Monks;K. Law;D. Ridley;S. Turquety;S. Tilmes;Jennie L. Thomas;I. Bouarar;J. Flemming;V. Huijnen;J. Mao;B. Duncan;S. Steenrod;Y. Yoshida;J. Langner;Y. Long
抽象。2008年7月，我们利用POLMIP多模式比较演习中的10个全球化学传输模式模拟，评估了高纬度地区（> 50° N）以生物质燃烧排放为主的对流层臭氧增强情况。在以火灾排放为主的模式空气质量中，受火灾影响的新鲜空气中的ΔO3/ΔCO值介于0.039和0.196 ppbv ppbv−1之间（平均值：0.113 ppbv ppbv−1），而受火灾影响的较老空气中的Δ O3/Δ CO值介于0.140和0.261 ppbv ppbv−1之间（平均值：0.193 ppbv）。这些值与文献中的观测估计值范围广泛一致。根据用于驱动模型的气象数据，模型ΔPAN/ΔCO增强比率显示出不同的分组。ECMWF强迫模式产生的ΔPAN/ΔCO值（4.47 ~ 7.00 pptv ppbv−1）大于GEOS 5强迫模式（1.87 ~ 3.28 pptv ppbv−1），我们发现这可能与中纬度源区向极地输出过程中垂直输送效率的差异有关。使用拉格朗日化学传输模型模拟了大量的生物质燃烧羽流和从北极输出的人为排放，结果表明，4天羽流中的臭氧净变化对POLMIP模型中羽流化学成分和羽流垂直位置的差异很敏感。特别是，北极臭氧演变的羽是高度敏感的PAN的初始浓度，以及含氧的挥发性有机化合物（丙酮，乙醛），由于它们在生产过氧乙酰基PAN前体的作用。垂直位移也是重要的，因为它对PAN的稳定性的影响，以及随后对NOx丰度的影响。在羽流中的净臭氧生产是有限的，我们发现，在羽流中的臭氧的寿命是敏感的过氧化氢负载，由于生产的HOx从过氧化物光解，和HO 2 + O3在控制臭氧损失的关键作用。总的来说，我们的研究结果表明，生物质燃烧排放导致大规模的光化学增强高纬度对流层臭氧在夏季。
Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high latitudes (> 50° N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, ΔO3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.47 to 7.00 pptv ppbv−1) than GEOS5-forced models (1.87 to 3.28 pptv ppbv−1), which we show is likely linked to differences in efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from towards the Arctic using a Lagrangian chemical transport model show that 4-day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HOx from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high-latitude tropospheric ozone during summer.